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This study examined perceived environmental and personal factors associated with walking and cycling as means of transportation for Taiwanese adults. A random-digit-dialing telephone-based cross-sectional survey was conducted with Taiwanese adults aged 20 to 64 years. Data on time spent walking and cycling for transportation and perceptions of neighborhood environment and personal characteristics were obtained from 1065 adults by using the International Physical Activity Questionnaire-long version and its environmental module. Adjusted binary logistic regression was performed. The results showed that, after adjusting potential confounders, common and different personal and perceived environmental factors were associated with walking and cycling for transportation. For common personal factors, adults who had employment were less likely to engage in 150 min of walking per week (odds ratio [OR] = 0.41; 95% confidence interval (CI): 0.27–0.62) and to use cycling as a means of transportation (OR = 0.51; 95% CI: 0.32–0.79). For common perceived environmental factors, adults who perceived good connectivity of streets were more likely to walk (OR = 1.95; 95% CI: 1.20–3.16) and cycle (OR = 2.02; 95% CI: 1.16–3.54) for transportation. Targeting employed adults and improving the connectivity of streets should be a priority for developing transport policies and intervention strategies to promote active transportation. Full article